As American involvement in the Vietnam War began, the A-1 Skyraider was still the medium attack aircraft in many carrier air wings, although it was planned to be replaced by the A-6A Intruder as part of the general switch to jet aircraft. Skyraiders from the carriers USS Constellation and Ticonderoga participated in the first U.S. Navy strikes against North Vietnam on 5 August 1964 as part of Operation Pierce Arrow in response to the Gulf of Tonkin Incident, striking against fuel depots at Vinh, with one Skyraider from Ticonderoga damaged by anti-aircraft fire, and a second from Constellation shot down, killing its pilot. During the war, U.S. Navy Skyraiders shot down two North Vietnamese Air Force (NVAF) Mig-17 Fresco jet fighters: one on 20 June 1965, a victory shared by Lieutenant Clinton B. Johnson and Lieutenant, junior grade Charles W. Hartman III of VA-25 and one on 9 October 1966 by LTJG William T. Patton of VA-176. While on his very first mission, Navy pilot Lieutenant (j.g.) Dieter Dengler took damage to his A-1H over Vietnam on 1 February 1966, and crash-landed in Laos.

As they were released from Navy service, Skyraiders were introduced into the South Vietnam Air Force (VNAF). They were also used by the USAF to perform one of the Skyraider's most famous roles: the "Sandy" helicopter escort on combat rescues. USAF Major Bernard F.Fisher piloted an A-1E on the 10 March 1966 mission for which he was awarded the Medal of Honor for rescuing Major "Jump" Myers at A Shau Special Forces Camp. USAF Colonel William A.Jones, III piloted an A-1H on the 1 September 1968 mission for which he was awarded the Medal of Honor. In that mission, despite damage to his aircraft and suffering serious burns, he returned to his base and reported the position of a downed U.S. airman.

After November 1972, all A-1s in U.S. service in Southeast Asia were transferred to the South Vietnamese Air Force (VNAF) and their roles taken over by the subsonic LTV A-7 corsair II. The Skyraider in Vietnam pioneered the concept of tough, survivable aircraft with long loiter times and large ordnance loads. The USAF lost 201 Skyraiders to all causes in Southeast Asia, while the Navy lost 65 to all causes. Of the 266 lost A-1s, five were shot down by surface-to-air missiles (SAMs), and three were shot down in air-to-air combat; two by North Vietnamese MiG-17s. The first A-1 was shot down on 29 April 1966, and the second A-1 was lost on 19 April 1967; both were from the 602 Air Commando Squadron (ACS). The third A-1 Skyraider was from Squadron VA-35 and was lost to a Chinese Mig-19 ( J-6) on 14 February 1968. Lieutenant (j.g.) Joseph P. Dunn, USN, had flown too close to the Chinese held island of Hainan, and had been intercepted. Lieutenant Dunn's A-1 Skyraider was the last U.S. Navy A-1 lost in the war. He did not survive. Shortly thereafter, A-1 Skyraider naval squadrons transitioned to the A-6 Intruder, A-7 Corsair II or Douglas A-4 Skyhawk.

In contrast to the Korean War, fought a decade earlier, the U.S. Air Force used the naval A-1 Skyraider for the first time in Vietnam. As the Vietnam War progressed, USAF A-1s were painted in camouflage, while USN A-1 Skyraiders were gray/white in color; again, in contrast to the Korean War, when A-1s were painted dark blue.

In October 1965, to highlight the dropping of the six millionth pound of ordnance, Commander Clarence J. Stoddard of Attack Squadron 25(VA-25), flying an A-1H, dropped a special, one-time only, object in addition to his other munitions – a toilet

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